Selective hydrogenation of 1,3-butadiene catalyzed by a single Pd atom anchored on graphene: the importance of dynamics.

ABSTRACT: The active-site structure, reaction mechanism, and product selectivity of the industrially important selective hydrogenation of 1,3-butadiene are investigated using first principles for an emerging single-atom Pd catalyst anchored on graphene. Density functional theory calculations suggest that the mono-π-adsorbed reactant undergoes sequential hydrogenation by Pd-activated H₂. Importantly, the high selectivity towards 1-butene is attributed to the post-transition-state dynamics in the second hydrogenation step, which leads exclusively to the desorption of the product. This dynamical event prevails despite the existence of energetically preferred 1-butene adsorption on Pd, which would eventually lead to complete hydrogenation to butane and be thus inconsistent with experimental o

SUBMITTER: Feng Y 

PROVIDER: S-EPMC6050543 | biostudies-literature | 2018 Jul

REPOSITORIES: biostudies-literature